Efficient Hybrid Particle-Field Coarse-Grained Model of Polymer Filler Interactions: Multiscale Hierarchical Structure of Carbon Black Particles in Contact with Polyethylene

In the present study, we propose, validate, and give first applications for large-scale systems of coarse-grained models suitable for filler/polymer interfaces based on carbon black (CB) and polyethylene (PE). The computational efficiency of the proposed approach, based on hybrid particle-field models (hPF), allows large-scale simulations of CB primary particles of realistic size (similar to 20 nm) embedded in PE melts. The molecular detailed models, here introduced, allow a microscopic description of the bound layer, through the analysis of the conformational behavior of PE chains adsorbed on different surface sites of CB primary particles, where the conformational behavior of adsorbed chains is different from models based on flat infinite surfaces. On the basis of the features of the systems, an optimized version of OCCAM code for large-scale (up to more than 8 million of beads) parallel runs is proposed and benchmarked. The computational efficiency of the proposed approach opens the possibility of a computational screening of the bound layer, involving the optimal combination of surface chemistry, size, and shape of CB aggregates and the molecular weight distribution of the polymers achieving an important tool to address the polymer/fillers interface and interphase engineering in the polymer industry.

Automated summary

The study introduces large-scale coarse-grained models for filler/polymer interfaces based on carbon black (CB) and polyethylene (PE) and validates their computational efficiency. The molecular models allow a description of PE chain conformational behavior adsorbed on CB primary particles. The proposed method opens up the possibility of a computational screening for optimal polymer/fillers interface and interphase engineering.